The coronavirus disease 2019 (COVID-19) pandemic has exerted tremendous effects on the residents of and caregivers at long-term care facilities (LTCF). The combination of a vulnerable, aged population, staffing shortages, and inadequate resources in LTCF will cause a great negative impact in these sectors. Addressing the caregiver’s lack of interest in providing care for patients with COVID-19 is a great challenge for institutional managers. The primary objective of this study was to analyze the factors related to the willingness of personnel at LTCF to provide care to patients with COVID-19. This was a cross-sectional study in which personnel from 10 LTCF were recruited as participants through convenience sampling and completed structured questionnaires. A total of 500 questionnaires were distributed and 385 valid questionnaires were recovered, posting a response rate of 77%. A statistical analysis was performed using SPSS 22.0. The results of the survey revealed that only 30% of the participants were willing to provide care to patients with COVID-19; 23% more of the participants were willing to provide such care if their institutions provided sufficient PPE. Regarding other conditions, 31.5% and 76% of the participants expressed that they would be willing to provide such care if their compensation were increased and working hours were reduced. In the univariate analysis, the willingness of participants with different characteristics (job categories, years of holding a professional certificate, job location type, monthly income, experience with caring for patients with confirmed COVID-19, and completion of training related to communicable disease control) varied significantly (p < 0.05). Furthermore, in the logistic regression analysis, several demographic and professional characteristics (education level, job category, number of patients served daily, and monthly income) were significantly correlated with willingness to provide care to patients with COVID-19 (p < 0.05). On the basis of these findings, the LTCF should securitize the associated factors of care wiliness in personnel to eliminate the difference of the willingness to provide care to patients with suspected or confirmed COVID-19.